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DOE OSTI2023

Impact of Pendent Ammonium Groups on Solubility and Cycling Charge Carrier Performance in Nonaqueous Redox Flow Batteries

The synthesis, characterization, electrochemical performance, and theoretical modeling of two base-metal charge carrier complexes incorporating a pendent quaternary ammonium group, [Ni(bppn-Me3)][BF4], 3′, and [Fe(PyTRENMe)][OTf]3, 4’, are described. Both complexes were produced in high yield and fully characterized using NMR, IR, and UV–vis spectroscopies as well as elemental analysis and single-crystal X-ray crystallography. The solubility of 3′ in acetonitrile showed a 283% improvement over its neutral precursor, whereas the solubility of complex 4’ was effectively unchanged. Cyclic voltammetry indicates an ∼0.1 V positive shift for all waves, with some changes in reversibility depending on the wave. Bulk electrochemical cycling demonstrates that both 3′ and 4’ can utilize the second more negative wave to a degree, whereas 4’ ceases to have a reversible positive wave. Flow cell testing of 3′ and 4’ with Fc as the posolyte reveals little improvement to the cycling performance of 3′ compared with its parent complex, whereas 4’ exhibits reductions in capacity decay when cycling either negative wave. Postcycling CVs indicate that crossover is the likely source of capacity loss in complexes 3, 3′, and 4’ because there is little change in the CV trace. Density functional theory calculations indicate that the ammonium group lowers the HOMO energy in 3′ and 4’, which may impart stability to cycling negative waves while making positive waves less accessible. The incorporation of a positively charged species can improve solubility, stored electron density, and capacity decay depending on the complex, features critical to high energy density redox flow battery performance.

25 ENERGY STORAGE↗

NASA NTRS2024

High Yield Exfoliation of a Sub-Micron Hexagonal Boron Nitride Using a Solvent Free Method

Sodium fluoride (NaF) has been found to be an activation agent in exfoliating a hexagonal boron nitride (hBN) platelet, using solvent free method. The procedure was carried out by enhancing the intercalation of ferric chloride (FeCl3) in an intermediate step, up to 330 °C, followed by removal of the by-product at room temperature. In this research, five additional common salts including lithium fluoride, potassium fluoride, lithium chloride, sodium chloride, and potassium chloride, were examined and compared to NaF for their effectiveness in producing the most exfoliation of a commercially available sub-micron-size hBN. It was found that, all fluoride and chloride salts significantly activated the intercalation of FeCl3 into this hBN. Analyses and characterization from X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy and Raman spectroscoy revealed NaCl to be one of most effective agents without further heat treatment and the least expensive salt in the intercalating reaction and exfoliation process. The synthetic route of this solvent free method is straightforward with 89% yield and above which can be produced on a large scale.

boron nitride↗

DOE OSTI2024

Profiling expression strategies for a type III polyketide synthase in a lysate-based, cell-free system

Abstract Some of the most metabolically diverse species of bacteria (e.g., Actinobacteria) have higher GC content in their DNA, differ substantially in codon usage, and have distinct protein folding environments compared to tractable expression hosts like Escherichia coli . Consequentially, expressing biosynthetic gene clusters (BGCs) from these bacteria in E. coli often results in a myriad of unpredictable issues with regard to protein expression and folding, delaying the biochemical characterization of new natural products. Current strategies to achieve soluble, active expression of these enzymes in tractable hosts can be a lengthy trial-and-error process. Cell-free expression (CFE) has emerged as a valuable expression platform as a testbed for rapid prototyping expression parameters. Here, we use a type III polyketide synthase from Streptomyces griseus , RppA, which catalyzes the formation of the red pigment flaviolin, as a reporter to investigate BGC refactoring techniques. We applied a library of constructs with different combinations of promoters and rppA coding sequences to investigate the synergies between promoter and codon usage. Subsequently, we assess the utility of cell-free systems for prototyping these refactoring tactics prior to their implementation in cells. Overall, codon harmonization improves natural product synthesis more than traditional codon optimization across cell-free and cellular environments. More importantly, the choice of coding sequences and promoters impact protein expression synergistically, which should be considered for future efforts to use CFE for high-yield protein expression. The promoter strategy when applied to RppA was not completely correlated with that observed with GFP, indicating that different promoter strategies should be applied for different proteins. In vivo experiments suggest that there is correlation, but not complete alignment between expressing in cell free and in vivo. Refactoring promoters and/or coding sequences via CFE can be a valuable strategy to rapidly screen for catalytically functional production of enzymes from BCGs, which advances CFE as a tool for natural product research.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Sparse expansions of multicomponent oxide configuration energy using coherency and redundancy

We report that compressed sensing has become a widely accepted paradigm to construct high dimensional cluster expansion models used for statistical mechanical studies of atomic configuration in complex multicomponent crystalline materials. However, strict sampling requirements necessary to obtain minimal coherence measurements for compressed sensing to guarantee accurate estimation of model parameters are difficult and in some cases impossible to satisfy due to the inability of physical systems to access certain configurations. Nevertheless, the dependence of energy on atomic configuration can still be adequately learned without these strict requirements by using compressed sensing by way of coherent measurements using redundant function sets known as frames. We develop a particular frame constructed from the union of all occupancy-based cluster expansion basis sets. We illustrate how using this highly redundant frame yields sparse expansions of the configuration energy of complex oxide materials that are competitive and often surpass the prediction accuracy and sparsity of models obtained from standard cluster expansions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Electrodeposition method development for Californium Rare Isotope Breeder Upgrade (CARIBU) Source

Electrodeposition is one of the most widely utilized techniques for thin-film production with high yields. Although it is used extensively, this technique still presents several issues limiting its usefulness, including excess thickness and frequent cracking of deposited films. Efforts to improve thin-film production recently undertaken at Oak Ridge Laboratory by the authors have included studying operating conditions and applied electrolytes. Samarium was used as a surrogate material for californium, and yield was compared with different deposition condition. The final procedure from the optimized condition will be applied during production of the californium-252 source for the Californium Rare Isotope Breeder Upgrade (CARIBU) project, and the fission fragment will be analyzed.

07 ISOTOPE AND RADIATION SOURCES↗

NASA NTRS1975

Reactively sputtered thin film photovoltaic devices

The feasibility of a reactively sputtered thin film CdS - Cu2S solar cell is proven. Identification of the reactively sputtered Cu2S film is made by X-ray diffractometer and spectro-transmission measurements. Because of its simplicity, economical use of material, and high yield, the reactive sputtering process promises to be a low cost method for producing CdS - Cu2S solar cells.

Hsieh, E. J.↗

NASA NTRS1982

Synthesis and characterization of bisimide amines and bisimide amine-cured epoxy resins

A study has been conducted with the objective of developing tough, moisture resistant, high char yield epoxy resins using novel bisimide amine (BIA) hardeners as curing agents with MY-720, a commercial state-of-the-art epoxy resin system. BIA cured epoxies are shown to have lower moisture absorption than MY-720 and other state-of-the-art epoxy resins; the tensile strengths and strain-to-failures of several of the bisimide epoxy resins (IME's) are higher than those of the state-of-the-art epoxies. Most IME's have compression properties equivalent to those of state-of-the-art epoxies. Two resin systems, IME-10 and IME-12-3, have better overall properties than other resin systems investigated.

Scola, D. A.↗

NASA NTRS2016

Monitoring Interannual Variation in Global Crop Yield Using Long-Term AVHRR and MODIS Observations

Advanced Very High Resolution Radiometer (AVHRR) and Moderate Resolution Imaging Spectroradiometer (MODIS) data have been extensively applied for crop yield prediction because of their daily temporal resolution and a global coverage. This study investigated global crop yield using daily two band Enhanced Vegetation Index (EVI2) derived from AVHRR (1981-1999) and MODIS (2000-2013) observations at a spatial resolution of 0.05deg (approx.5 km). Specifically, EVI2 temporal trajectory of crop growth was simulated using a hybrid piecewise logistic model (HPLM) for individual pixels, which was used to detect crop phenological metrics. The derived crop phenology was then applied to calculate crop greenness defined as EVI2 amplitude and EVI2 integration during annual crop growing seasons, which was further aggregated for croplands in each country, respectively. The interannual variations in EVI2 amplitude and EVI2 integration were combined to correlate to the variation in cereal yield from 1982-2012 for individual countries using a stepwise regression model, respectively. The results show that the confidence level of the established regression models was higher than 90% (P value < 0.1) in most countries in the northern hemisphere although it was relatively poor in the southern hemisphere (mainly in Africa). The error in the yield predication was relatively smaller in America, Europe and East Asia than that in Africa. In the 10 countries with largest cereal production across the world, the prediction error was less than 9% during past three decades. This suggests that crop phenology-controlled greenness from coarse resolution satellite data has the capability of predicting national crop yield across the world, which could provide timely and reliable crop information for global agricultural trade and policymakers.

Crop phenology↗

NASA NTRS1987

A mathematical model of a lithium/thionyl chloride primary cell

A 1-D mathematical model for the lithium/thionyl chloride primary cell was developed to investigate methods of improving its performance and safety. The model includes many of the components of a typical lithium/thionyl chloride cell such as the porous lithium chloride film which forms on the lithium anode surface. The governing equations are formulated from fundamental conservation laws using porous electrode theory and concentrated solution theory. The model is used to predict 1-D, time dependent profiles of concentration, porosity, current, and potential as well as cell temperature and voltage. When a certain discharge rate is required, the model can be used to determine the design criteria and operating variables which yield high cell capacities. Model predictions can be used to establish operational and design limits within which the thermal runaway problem, inherent in these cells, can be avoided.

Evans, T. I.↗

DOE OSTI2025

Predicting weather impacts on corn production in a data-limited region using a transfer learning approach

The stability of food supply and prices may depend more on annual changes in yields from year-to-year variability in weather than on longer-term average changes from changing climatic conditions. However, the absence of high-quality data on crop yields at fine spatial resolutions in many regions of the world makes it challenging to statistically model their response to interannual variability in weather patterns. Therefore, there is a need for empirical methods that can project annual crop yield changes even in limited data regions. Here, we propose a transfer learning algorithm that uses high spatial resolution data from one region to project yields in another region with more limited data. The goal of our work is to understand what data types can be beneficial for transferring learning from a source region to a very different target region with more limited data. We utilize Long Short-Term Memory to develop a transfer learning model that is trained on historical county-level corn yield in the United States and predicts district-level corn yield variations in India. Even using smaller amounts of data in India, simulating a data-scarce region, we achieve an average root mean square error of 0.48 bu acre−1 in predicting interannual yield variations. Using Shapley values to interpret results, we explore the contribution of the different weather parameters to interannual yield variability and find a larger influence of precipitation-related variables. Our study demonstrates the usefulness of this method for transferring models of weather impacts on crop yields trained on a data-rich country to one with more limited data. It suggests the potential of applying the transfer learning model to mitigate the need for extensive raw data globally.

Vishwakarma, Srishti [ORNL] (ORCID:000000031674419↗

NASA NTRS1988

Velocity-pressure integrated versus penalty finite element methods for high Reynolds number flows

Velocity-pressure integrated and consistent penalty finite element computations of high Reynolds number, laminar flows are presented. In both of the methods, the pressure has been interpolated using linear shape functions for a triangular element. The triangular element is contained inside the bi-quadratic isoparametric element. It has been reported previously that the pressure interpolation method, when used in the velocity-pressure integrated method, yielded accurate computational results for high Reynolds number flows. It is shown that use of the same pressure interpolation method in the consistent penalty finite element method yielded accurate velocity and pressure fields which were comparable to those obtained using the velocity-pressure integrated method. Accuracy of the two finite element methods has been demonstrated by comparing the computational results with available experimental data and/or fine-grid finite difference computational results. Advantages and disadvantages of the two methods are discussed on the basis of accuracy and convergence nature. Example problems considered include a lid-driven cavity flow for Reynolds number of 10,000, a laminar backward-facing step flow, a laminar flow through a nest of cylinders, and a channel flow with an internal blockage. A finite element computer program (NSFLOW/P) for the 2-D, incompressible Navier-Stokes equations is also presented.

Kim, Sang-Wook↗

DOE OSTI2025

Wind Turbine Rotor Design Using High-Fidelity Aerostructural Optimization

Large wind turbines yield more energy but demand careful aeroelastic blade design. Coupled multiphysics design strategies can reduce wind energy costs by exploiting fluid-structure interactions. This work presents the first high-fidelity aerostructural optimization study of a large wind turbine rotor. We use blade-resolved fluid dynamics and structural solvers in a monolithic gradient-based optimization framework to explore steady-state torque and blade mass tradeoffs. The coupled-adjoint approach computes gradients efficiently, enabling the optimization of over 100 structural and geometric parameters simultaneously. Our optimization study modifies a DTU 10 MW benchmark with a simplified structure and isotropic material properties. The tightly coupled optimizations increase torque by 14% while reducing rotor mass by 9% or reduce blade mass by 27% while maintaining torque. Blade-resolved models provide greater design freedom, enabling 5% higher mass reductions than conventional parameterizations at equal torque. This framework paves the way for more detailed high-fidelity optimization studies to complement conventional design approaches.

17 WIND ENERGY↗

DOE OSTI2024

Integrated Approach to CO 2 Capture and Conversion to Cyclic Carbonates under Solvent- and Additive-Free Conditions Utilizing the CO 2 Capture Solvent EEMPA

An integrated CO 2 capture and conversion to materials (IC 3 M) implementation utilizing a CO 2 capture solvent is an efficient approach to reduce the amount of CO 2 in the atmosphere while producing value-added chemicals. In this work, we demonstrate that the advanced water-lean CO 2 capture solvent, N-(2-Ethoxyethyl)-3-morpholinopropan-1-amine (EEMPA), can catalyze the cycloaddition reaction between CO 2 and propylene oxide to produce the value-added chemical propylene carbonate in an IC 3 M fashion. When excess propylene oxide is used relative to EEMPA, yields as high as 75% with 85% selectivity toward propylene carbonate can be achieved under solvent-free conditions without the need of additives/cocatalysts. The reaction temperature (120 °C) is comparable to that used in the thermal regeneration of the capture solvent under industrial conditions. Formation of an undesired amino alcohol side product was observed, but it may be reversible or avoidable with continued research despite the unsuccessful initial attempts. Finally, we show that this can be applied to other epoxides for the production of various cyclic carbonates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Voltage scanning and technical upgrades at the Collinear Resonance Ionization Spectroscopy experiment

To optimize the performance of the Collinear Resonance Ionization Spectroscopy (CRIS) experiment at CERN-ISOLDE, technical upgrades are continuously introduced, aiming to enhance its sensitivity, precision, stability, and efficiency. Recently, a voltage-scanning setup was developed and commissioned at CRIS, which improved the scanning speed by a factor of three as compared to the current laser-frequency scanning approach. This leads to faster measurements of the hyperfine structure for systems with high yields (more than a few thousand ions per second). Additionally, several beamline sections have been redesigned and manufactured, including a new field-ionization unit, an electrostatic bend with a larger deflection angle, and improved ion optics. The beamline upgrades are expected to yield an improvement of at least a factor of 5 in the signal-to-noise ratio by avoiding the use of high-power lasers (which yield non-resonantly produced ions) and providing time-of-flight separation between the resonant ions and the collisional background.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Evaluation of a 5kW Solid Oxide Electrolysis Cell Stack

Electrolysis is the process of combining water and energy to produce oxygen and hydrogen gas. A solid oxide electrolysis cell (SOEC) is a type of high-temperature electrochemical cell used to yield hydrogen from steam. Many of these cells are put together to form an SOEC stack which operates between 600°C and 1000°C. There are several electrochemical methods for producing hydrogen, but the benefit of high-temperature electrolysis (HTE) in SOECs is they exhibit very high electrical efficiency and the potential for harnessing excess heat from other industrial processes such as nuclear power generation, fertilizer production, and chemical production.

08 - HYDROGEN↗

NASA NTRS2007

Impacts of Urbanization in the Coastal Tropical City of San Juan, Puerto Rico

Urban sprawl in tropical locations is rapidly accelerating and it is more evident in islands where a large percentage of the population resides along the coasts. This paper focuses on the analysis of the impacts of land use and land cover for urbanization in the tropical coastal city of San Juan, in the Caribbean island of Puerto Rico. A mesoscale numerical model, the Regional Atmospheric Modeling System (RAMS), is used to study the impacts of land use for urbanization in the environment including specific characteristics of the urban heat island in the San Juan Metropolitan Area (SJMA), one of the most noticeable urban cores of the Caribbean. The research also makes use of the observations obtained during the airborne San Juan Atlas Mission. Surface and rawinsonde data from the mission are used to validate the atmospheric model yielding satisfactory results. Airborne high resolution remote sensing data are used to update the model's surface characteristics in order to obtain a more accurate and detailed configuration of the SJMA and perform a climate impact analysis based on land cover/land use (LCLU) changes. The impact analysis showed that the presence of the urban landscape of San Juan has an impact reflected in higher air temperatures over the area occupied by the city, with positive values of up to 2.5 C, for the simulations that have specified urban LCLU indexes in the model's bottom boundary. One interesting result of the impact analysis was the finding of a precipitation disturbance shown as a difference in total accumulated rainfall between the present urban landscape and with a potential natural vegetation, apparently induced by the presence of the urban area. Results indicate that the urban enhanced cloud formation and precipitation development occur mainly downwind of the city, including the accumulated precipitation. This spatial pattern can be explained by the presence of a larger urbanized area in the southwest sector of the city, and of the approaching northeasterly trade winds. No significant impacts were found in the sea breeze patterns of the city.

Comarazamy, Daniel E.↗

NASA NTRS2007

Impacts of Urbanization in the Coastal Tropical City of San Juan, Puerto Rico

Urban sprawl in tropical locations is rapidly accelerating and it is more evident in islands where a large percentage of the population resides along the coasts. This paper focuses on the analysis of the impacts of land use and land cover for urbanization in the tropical coastal city of San Juan, in the Caribbean island of Puerto Rico. A mesoscale numerical model, the Regional Atmospheric Modeling System (RAMS), is used to study the impacts of land use for urbanization in the environment including specific characteristics of the urban heat island in the San Juan Metropolitan Area (SJMA), one of the most noticeable urban cores of the Caribbean. The research also makes use of the observations obtained during the airborne San Juan Atlas Mission. Surface and raw insonde data from the mission are used to validate the atmospheric model yielding satisfactory results. Airborne high resolution remote sensing data are used to update the model's surface characteristics in order to obtain a more accurate and detailed configuration of the SJMA and perform a climate impact analysis based on land cover/land use (LCLU) changes. The impact analysis showed that the presence of the urban landscape of San Juan has an impact reflected in higher air temperatures over the area occupied by the city, with positive values of up to 2.5 degrees C, for the simulations that have specified urban LCLU indexes in the model's bottom boundary. One interesting result of the impact analysis was the finding of a precipitation disturbance shown as a difference in total accumulated rainfall between the present urban landscape and with a potential natural vegetation, apparently induced by the presence of the urban area. Results indicate that the urban-enhanced cloud formation and precipitation development occur mainly downwind of the city, including the accumulated precipitation. This spatial pattern can be explained by the presence of a larger urbanized area in the southwest sector of the city, and of the approaching northeasterly trade winds.

Comarazamy, Daniel E.↗

DOE OSTI2026

Separation of radium and actinium in acetic acid/acetate solutions using TK101 resin

Here, the uptake and elution behavior of Ra and Ac was studied on TK101 resin using acetic acid and acetate buffer (acetic acid/lithium acetate) solutions. There is high extraction of Ra (>10 3 ) over a wide range of acetic acid concentrations (0.02 to 4 M) with slightly lower extraction (>10 2 ) in the acetate buffer solutions (pH 3.9 to 5.6). The Ac extraction is considerably lower with a maximum D w of ∼100, and negligible extraction at high acetic acid concentrations (> 1 M) and in the acetate buffer solutions. The difference in D w can be leveraged for highly efficient separations of Ac from Ra, with no detectable Ra in the Ac fractions and high Ac yields (∼100%). These separations may be useful for radiopharmaceutical applications as the Ac purity is extremely high and the elution conditions can be optimized to be biologically safe and appropriate for chelation to molecules relevant to targeted alpha therapy.

and nuclear chemistry↗